Title: Exploratory study of atmospheric methane enhancements derived from natural gas use in the Houston urban area

Here, the extensive use of natural gas (NG) in urban areas for heating, cooking and as a vehicular fuel is associated with potentially significant emissions of methane (CH 4) to the atmosphere. Methane, a potent greenhouse gas that influences the chemistry of the atmosphere, can be emitted from different sources including leakage from NG infrastructure, transportation activities, end-use uncombusted NG, landfills and livestock. Although significant CH 4 leakage associated with aging local NG distribution systems in the U.S. has been reported, further investigation is required to study the role of this infrastructure component and other NG-related sources in atmospheric CH 4 enhancements in urban centers. In this study, neighborhood-scale mobile-based monitoring of potential CH 4 emissions associated with NG in the Greater Houston area (GHA) is reported. A novel dual-gas 3.337 μm interband cascade laser-based sensor system was developed and mobile-mode deployed for simultaneous CH 4 and ethane (C 2H 6) monitoring during a period of over 14 days, corresponding to ~ 90 hours of effective data collection during summer 2016. The sampling campaign covered ~ 250 road miles and was primarily concentrated on eight residential zones with distinct infrastructure age and NG usage levels. A moderate number of elevatedmore » CH 4 concentration events (37 episodes) with mixing ratios not exceeding 3.60 ppmv and associated with atmospheric background enhancements below 1.21 ppmv were observed during the field campaign. Source discrimination analyses based on the covariance between CH 4 and C 2H 6 levels indicated the predominance of thermogenic sources (e.g., NG) in the elevated CH 4 concentration episodes. The volumetric fraction of C 2H 6 in the sources associated with the thermogenic CH 4 spikes varied between 2.7 and 5.9%, concurring with the C 2H 6 content in NG distributed in the GHA. Isolated CH 4 peak events with significantly higher C 2H 6 enhancements (~11 %) were observed at industrial areas and locations with high density of petroleum and gas pipelines in the GHA, indicating potential variability in Houston’s thermogenic CH 4 sources.« less

@article{osti_1435611,
title = {Exploratory study of atmospheric methane enhancements derived from natural gas use in the Houston urban area},
author = {Sanchez, Nancy P. and Zheng, Chuantao and Ye, Weilin and Czader, Beata and Cohan, Daniel S. and Tittel, Frank K. and Griffin, Robert J.},
abstractNote = {Here, the extensive use of natural gas (NG) in urban areas for heating, cooking and as a vehicular fuel is associated with potentially significant emissions of methane (CH4) to the atmosphere. Methane, a potent greenhouse gas that influences the chemistry of the atmosphere, can be emitted from different sources including leakage from NG infrastructure, transportation activities, end-use uncombusted NG, landfills and livestock. Although significant CH4 leakage associated with aging local NG distribution systems in the U.S. has been reported, further investigation is required to study the role of this infrastructure component and other NG-related sources in atmospheric CH4 enhancements in urban centers. In this study, neighborhood-scale mobile-based monitoring of potential CH4 emissions associated with NG in the Greater Houston area (GHA) is reported. A novel dual-gas 3.337 μm interband cascade laser-based sensor system was developed and mobile-mode deployed for simultaneous CH4 and ethane (C2H6) monitoring during a period of over 14 days, corresponding to ~ 90 hours of effective data collection during summer 2016. The sampling campaign covered ~ 250 road miles and was primarily concentrated on eight residential zones with distinct infrastructure age and NG usage levels. A moderate number of elevated CH4 concentration events (37 episodes) with mixing ratios not exceeding 3.60 ppmv and associated with atmospheric background enhancements below 1.21 ppmv were observed during the field campaign. Source discrimination analyses based on the covariance between CH4 and C2H6 levels indicated the predominance of thermogenic sources (e.g., NG) in the elevated CH4 concentration episodes. The volumetric fraction of C2H6 in the sources associated with the thermogenic CH4 spikes varied between 2.7 and 5.9%, concurring with the C2H6 content in NG distributed in the GHA. Isolated CH4 peak events with significantly higher C2H6 enhancements (~11 %) were observed at industrial areas and locations with high density of petroleum and gas pipelines in the GHA, indicating potential variability in Houston’s thermogenic CH4 sources.},
doi = {10.1016/j.atmosenv.2018.01.001},
journal = {Atmospheric Environment (1994)},
number = C,
volume = 176,
place = {United States},
year = {2018},
month = {1}
}

A new, integrated methodology to locate and measure methane emissions from natural gas systems has been developed. Atmospheric methane sources are identified by elevated ambient CH{sub 4} concentrations meaured with a mobile laser-based methane analyzer. The total methane emission rate from a source is obtained by simulating the source with a sulfur hexafluoride (SF{sub 6}) tracer gas release and by measuring methane and tracer concentrations along downwind sampling paths using mobile, real-time analyzers. Combustion sources of methane are distinguished from noncombustion sources by concurrent ambient carbon dioxide measurements. Three variations on the tracer ratio method are described for application tomore » (1) small underground vaults, (2) above-ground natural gas facilities, and (3) diffuse methane emissions from an entire town. Results from controlled releases and from replicate tests demonstrate that the tracer ratio approach can yield total emission rates to within approximately {+-}15%. The estimated accuracy of emission estimates for urban areas with a variety of diffuse emissions is {+-}50%. 21 refs., 5 figs., 6 tabs.« less

Future energy systems may rely on natural gas as a low-cost fuel to support variable renewable power. However, leaking natural gas causes climate damage because methane (CH 4) has a high global warming potential. In this study, we use extreme-value theory to explore the distribution of natural gas leak sizes. By analyzing ~15,000 measurements from 18 prior studies, we show that all available natural gas leakage datasets are statistically heavy-tailed, and that gas leaks are more extremely distributed than other natural and social phenomena. A unifying result is that the largest 5% of leaks typically contribute over 50% of themore » total leakage volume. While prior studies used lognormal model distributions, we show that lognormal functions poorly represent tail behavior. Our results suggest that published uncertainty ranges of CH 4 emissions are too narrow, and that larger sample sizes are required in future studies to achieve targeted confidence intervals. Additionally, we find that cross-study aggregation of datasets to increase sample size is not recommended due to apparent deviation between sampled populations. Finally, understanding the nature of leak distributions can improve emission estimates, better illustrate their uncertainty, allow prioritization of source categories, and improve sampling design. Also, these data can be used for more effective design of leak detection technologies.« less

This study presents the results of a campaign that estimated methane emissions at 268 gas production facilities in the Fayetteville shale gas play using onsite measurements (261 facilities) and two downwind methods - the dual tracer flux ratio method (Tracer Facility Estimate - TFE, 17 facilities) and the EPA Other Test Method 33a (OTM33A Facility Estimate - OFE, 50 facilities). A study onsite estimate (SOE) for each facility was developed by combining direct measurements and simulation of unmeasured emission sources, using operator activity data and emission data from literature. The SOE spans 0-403 kg/h and simulated methane emissions from liquidmore » unloadings account for 88% of total emissions estimated by the SOE, with 76% (95% CI [51%-92%]) contributed by liquid unloading at two facilities. TFE and SOE show overlapping 95% CI between individual estimates at 15 of 16 (94%) facilities where the measurements were paired, while OFE and SOE show overlapping 95% CI between individual estimates at 28 of 43 (65%) facilities. However, variance-weighted least-squares (VWLS) regressions performed on sets of paired estimates indicate statistically significant differences between methods. The SOE represents a lower bound of emissions at facilities where onsite direct measurements of continuously emitting sources are the primary contributor to the SOE, a sub-selection of facilities which minimizes expected inter-method differences for intermittent pneumatic controllers and the impact of episodically-emitting unloadings. At 9 such facilities, VWLS indicates that TFE estimates systematically higher emissions than SOE (TFE-to-SOE ratio = 1.6, 95% CI [1.2 to 2.1]). At 20 such facilities, VWLS indicates that OFE estimates systematically lower emissions than SOE (OFE-to-SOE ratio of 0.41 [0.26 to 0.90]). Given that SOE at these facilities is a lower limit on emissions, these results indicate that OFE is likely a less accurate method than SOE or TFE for this type of facility.« less

Increased natural gas production in recent years has spurred intense interest in methane (CH 4) emissions associated with its production, gathering, processing, transmission, and distribution. Gathering and processing facilities (G&P facilities) are unique in that the wide range of gas sources (shale, coal-bed, tight gas, conventional, etc.) results in a wide range of gas compositions, which in turn requires an array of technologies to prepare the gas for pipeline transmission and distribution. We present an overview and detailed description of the measurement method and analysis approach used during a 20-week field campaign studying CH 4 emissions from the natural gasmore » G&P facilities between October 2013 and April 2014. Dual-tracer flux measurements and on-site observations were used to address the magnitude and origins of CH 4 emissions from these facilities. The use of a second tracer as an internal standard revealed plume-specific uncertainties in the measured emission rates of 20–47%, depending upon plume classification. Furthermore, combining downwind methane, ethane (C 2H 6), carbon monoxide (CO), carbon dioxide (CO 2), and tracer gas measurements with on-site tracer gas release allows for quantification of facility emissions and in some cases a more detailed picture of source locations.« less

Divergence in recent oil and gas related methane emission estimates between aircraft studies (basin total for a midday window) and emissions inventories (annualized regional and national statistics) indicate the need for better understanding the experimental design, including temporal and spatial alignment and interpretation of results. In our aircraft-based methane emission estimates in a major U.S. shale gas basin resolved from west to east show (i) similar spatial distributions for 2 days, (ii) strong spatial correlations with reported NG production (R 2 = 0.75) and active gas well pad count (R 2 = 0.81), and (iii) 2× higher emissions in themore » western half (normalized by gas production) despite relatively homogeneous dry gas and well characteristics. Operator reported hourly activity data show that midday episodic emissions from manual liquid unloadings (a routine operation in this basin and elsewhere) could explain ~1/3 of the total emissions detected midday by the aircraft and ~2/3 of the west–east difference in emissions. The 22% emission difference between both days further emphasizes that episodic sources can substantially impact midday methane emissions and that aircraft may detect daily peak emissions rather than daily averages that are generally employed in emissions inventories. And while the aircraft approach is valid, quantitative, and independent, this study sheds new light on the interpretation of previous basin scale aircraft studies, and provides an improved mechanistic understanding of oil and gas related methane emissions.« less